Epitaxial Ferroelectric Hf0.5Zr0.5O2 with Metallic Pyrochlore Oxide Electrodes

Zimeng Zhang; Shang Lin Hsu; Vladimir A. Stoica; Hanjong Paik; Eric Parsonnet; Alexander Qualls; Jianjun Wang; Liang Xie; Mukesh Kumari; Sujit Das; Zhinan Leng; Martin McBriarty; Roger Proksch; Alexei Gruverman; Darrell G. Schlom; Long Qing Chen; Sayeef Salahuddin; Lane W. Martin; Ramamoorthy Ramesh

doi:10.1002/adma.202006089

Epitaxial Ferroelectric Hf_0.5Zr_0.5O₂ with Metallic Pyrochlore Oxide Electrodes

Zimeng Zhang, Shang Lin Hsu, Vladimir A. Stoica, Hanjong Paik, Eric Parsonnet, Alexander Qualls, Jianjun Wang, Liang Xie, Mukesh Kumari, Sujit Das, Zhinan Leng, Martin McBriarty, Roger Proksch, Alexei Gruverman, Darrell G. Schlom, Long Qing Chen, Sayeef Salahuddin, Lane W. Martin, Ramamoorthy Ramesh

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Abstract

The synthesis of fully epitaxial ferroelectric Hf_0.5Zr_0.5O₂ (HZO) thin films through the use of a conducting pyrochlore oxide electrode that acts as a structural and chemical template is reported. Such pyrochlores, exemplified by Pb₂Ir₂O₇(PIO) and Bi₂Ru₂O₇(BRO), exhibit metallic conductivity with room-temperature resistivity of <1 mΩ cm and are closely lattice matched to yttria-stabilized zirconia substrates as well as the HZO layers grown on top of them. Evidence for epitaxy and domain formation is established with X-ray diffraction and scanning transmission electron microscopy, which show that the c-axis of the HZO film is normal to the substrate surface. The emergence of the non-polar-monoclinic phase from the polar-orthorhombic phase is observed when the HZO film thickness is ≥≈30 nm. Thermodynamic analyses reveal the role of epitaxial strain and surface energy in stabilizing the polar phase as well as its coexistence with the non-polar-monoclinic phase as a function of film thickness.

Original language	English (US)
Article number	2006089
Journal	Advanced Materials
Volume	33
Issue number	10
DOIs	https://doi.org/10.1002/adma.202006089
State	Published - Mar 11 2021

All Science Journal Classification (ASJC) codes

General Materials Science
Mechanics of Materials
Mechanical Engineering

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10.1002/adma.202006089

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Zhang, Z., Hsu, S. L., Stoica, V. A., Paik, H., Parsonnet, E., Qualls, A., Wang, J., Xie, L., Kumari, M., Das, S., Leng, Z., McBriarty, M., Proksch, R., Gruverman, A., Schlom, D. G., Chen, L. Q., Salahuddin, S., Martin, L. W., & Ramesh, R. (2021). Epitaxial Ferroelectric Hf_0.5Zr_0.5O₂ with Metallic Pyrochlore Oxide Electrodes. Advanced Materials, 33(10), Article 2006089. https://doi.org/10.1002/adma.202006089

@article{35625fda841843a49a1086cc8ded2ba4,

title = "Epitaxial Ferroelectric Hf0.5Zr0.5O2 with Metallic Pyrochlore Oxide Electrodes",

abstract = "The synthesis of fully epitaxial ferroelectric Hf0.5Zr0.5O2 (HZO) thin films through the use of a conducting pyrochlore oxide electrode that acts as a structural and chemical template is reported. Such pyrochlores, exemplified by Pb2Ir2O7(PIO) and Bi2Ru2O7(BRO), exhibit metallic conductivity with room-temperature resistivity of <1 mΩ cm and are closely lattice matched to yttria-stabilized zirconia substrates as well as the HZO layers grown on top of them. Evidence for epitaxy and domain formation is established with X-ray diffraction and scanning transmission electron microscopy, which show that the c-axis of the HZO film is normal to the substrate surface. The emergence of the non-polar-monoclinic phase from the polar-orthorhombic phase is observed when the HZO film thickness is ≥≈30 nm. Thermodynamic analyses reveal the role of epitaxial strain and surface energy in stabilizing the polar phase as well as its coexistence with the non-polar-monoclinic phase as a function of film thickness.",

author = "Zimeng Zhang and Hsu, {Shang Lin} and Stoica, {Vladimir A.} and Hanjong Paik and Eric Parsonnet and Alexander Qualls and Jianjun Wang and Liang Xie and Mukesh Kumari and Sujit Das and Zhinan Leng and Martin McBriarty and Roger Proksch and Alexei Gruverman and Schlom, {Darrell G.} and Chen, {Long Qing} and Sayeef Salahuddin and Martin, {Lane W.} and Ramamoorthy Ramesh",

note = "Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2021",

month = mar,

day = "11",

doi = "10.1002/adma.202006089",

language = "English (US)",

volume = "33",

journal = "Advanced Materials",

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Zhang, Z, Hsu, SL, Stoica, VA, Paik, H, Parsonnet, E, Qualls, A, Wang, J, Xie, L, Kumari, M, Das, S, Leng, Z, McBriarty, M, Proksch, R, Gruverman, A, Schlom, DG, Chen, LQ, Salahuddin, S, Martin, LW & Ramesh, R 2021, 'Epitaxial Ferroelectric Hf_0.5Zr_0.5O₂ with Metallic Pyrochlore Oxide Electrodes', Advanced Materials, vol. 33, no. 10, 2006089. https://doi.org/10.1002/adma.202006089

TY - JOUR

T1 - Epitaxial Ferroelectric Hf0.5Zr0.5O2 with Metallic Pyrochlore Oxide Electrodes

AU - Zhang, Zimeng

AU - Hsu, Shang Lin

AU - Stoica, Vladimir A.

AU - Paik, Hanjong

AU - Parsonnet, Eric

AU - Qualls, Alexander

AU - Wang, Jianjun

AU - Xie, Liang

AU - Kumari, Mukesh

AU - Das, Sujit

AU - Leng, Zhinan

AU - McBriarty, Martin

AU - Proksch, Roger

AU - Gruverman, Alexei

AU - Schlom, Darrell G.

AU - Chen, Long Qing

AU - Salahuddin, Sayeef

AU - Martin, Lane W.

AU - Ramesh, Ramamoorthy

PY - 2021/3/11

Y1 - 2021/3/11

N2 - The synthesis of fully epitaxial ferroelectric Hf0.5Zr0.5O2 (HZO) thin films through the use of a conducting pyrochlore oxide electrode that acts as a structural and chemical template is reported. Such pyrochlores, exemplified by Pb2Ir2O7(PIO) and Bi2Ru2O7(BRO), exhibit metallic conductivity with room-temperature resistivity of <1 mΩ cm and are closely lattice matched to yttria-stabilized zirconia substrates as well as the HZO layers grown on top of them. Evidence for epitaxy and domain formation is established with X-ray diffraction and scanning transmission electron microscopy, which show that the c-axis of the HZO film is normal to the substrate surface. The emergence of the non-polar-monoclinic phase from the polar-orthorhombic phase is observed when the HZO film thickness is ≥≈30 nm. Thermodynamic analyses reveal the role of epitaxial strain and surface energy in stabilizing the polar phase as well as its coexistence with the non-polar-monoclinic phase as a function of film thickness.

AB - The synthesis of fully epitaxial ferroelectric Hf0.5Zr0.5O2 (HZO) thin films through the use of a conducting pyrochlore oxide electrode that acts as a structural and chemical template is reported. Such pyrochlores, exemplified by Pb2Ir2O7(PIO) and Bi2Ru2O7(BRO), exhibit metallic conductivity with room-temperature resistivity of <1 mΩ cm and are closely lattice matched to yttria-stabilized zirconia substrates as well as the HZO layers grown on top of them. Evidence for epitaxy and domain formation is established with X-ray diffraction and scanning transmission electron microscopy, which show that the c-axis of the HZO film is normal to the substrate surface. The emergence of the non-polar-monoclinic phase from the polar-orthorhombic phase is observed when the HZO film thickness is ≥≈30 nm. Thermodynamic analyses reveal the role of epitaxial strain and surface energy in stabilizing the polar phase as well as its coexistence with the non-polar-monoclinic phase as a function of film thickness.

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U2 - 10.1002/adma.202006089

DO - 10.1002/adma.202006089

M3 - Article

C2 - 33533113

AN - SCOPUS:85100192756

SN - 0935-9648

VL - 33

JO - Advanced Materials

JF - Advanced Materials

IS - 10

M1 - 2006089

ER -

Epitaxial Ferroelectric Hf_0.5Zr_0.5O₂ with Metallic Pyrochlore Oxide Electrodes

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